Enhanced rare-earth separation with a metal-sensitive lanmodulin dimer.

Autor: Mattocks JA; Department of Chemistry, The Pennsylvania State University, University Park, PA, USA., Jung JJ; Department of Chemistry, The Pennsylvania State University, University Park, PA, USA., Lin CY; Department of Chemistry, The Pennsylvania State University, University Park, PA, USA., Dong Z; Critical Materials Institute, Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, Livermore, CA, USA., Yennawar NH; The Huck Institutes of the Life Sciences, The Pennsylvania State University, University Park, PA, USA., Featherston ER; Department of Chemistry, The Pennsylvania State University, University Park, PA, USA., Kang-Yun CS; Critical Materials Institute, Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, Livermore, CA, USA., Hamilton TA; Department of Chemistry, The Pennsylvania State University, University Park, PA, USA., Park DM; Critical Materials Institute, Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, Livermore, CA, USA. park36@llnl.gov., Boal AK; Department of Chemistry, The Pennsylvania State University, University Park, PA, USA. akb20@psu.edu.; Department of Biochemistry and Molecular Biology, The Pennsylvania State University, University Park, PA, USA. akb20@psu.edu., Cotruvo JA Jr; Department of Chemistry, The Pennsylvania State University, University Park, PA, USA. juc96@psu.edu.
Jazyk: angličtina
Zdroj: Nature [Nature] 2023 Jun; Vol. 618 (7963), pp. 87-93. Date of Electronic Publication: 2023 May 31.
DOI: 10.1038/s41586-023-05945-5
Abstrakt: Technologically critical rare-earth elements are notoriously difficult to separate, owing to their subtle differences in ionic radius and coordination number 1-3 . The natural lanthanide-binding protein lanmodulin (LanM) 4,5 is a sustainable alternative to conventional solvent-extraction-based separation 6 . Here we characterize a new LanM, from Hansschlegelia quercus (Hans-LanM), with an oligomeric state sensitive to rare-earth ionic radius, the lanthanum(III)-induced dimer being >100-fold tighter than the dysprosium(III)-induced dimer. X-ray crystal structures illustrate how picometre-scale differences in radius between lanthanum(III) and dysprosium(III) are propagated to Hans-LanM's quaternary structure through a carboxylate shift that rearranges a second-sphere hydrogen-bonding network. Comparison to the prototypal LanM from Methylorubrum extorquens reveals distinct metal coordination strategies, rationalizing Hans-LanM's greater selectivity within the rare-earth elements. Finally, structure-guided mutagenesis of a key residue at the Hans-LanM dimer interface modulates dimerization in solution and enables single-stage, column-based separation of a neodymium(III)/dysprosium(III) mixture to >98% individual element purities. This work showcases the natural diversity of selective lanthanide recognition motifs, and it reveals rare-earth-sensitive dimerization as a biological principle by which to tune the performance of biomolecule-based separation processes.
(© 2023. The Author(s).)
Databáze: MEDLINE
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